相关论文: Making Many-Body Interactions Nearly Pairwise Addi…
The many-body expansion (MBE) is an efficient tool which has a long history of use for calculating interaction energies, binding energies, lattice energies, and so on. In the past, applications of MBE to correlation energy have been…
Fragmentation methods such as the many-body expansion (MBE) are a common strategy to model large systems by partitioning energies into a hierarchy of decreasingly significant contributions. The number of fragments required for chemical…
We show how an embedded many-body expansion (EMBE) can be used to calculate accurate \emph{ab initio} energies of water clusters and ice structures using wavefunction-based methods. We use the EMBE described recently by Bygrave \emph{et…
The multipole-expansion (MPE) model is an implicit solvation model used to efficiently incorporate solvent effects in quantum chemistry. Even within the recent direct approach, the multipole basis used in MPE to express the dielectric…
The many-body expansion (MBE) of energies of molecular clusters or solids offers a way to detect and analyze errors of theoretical methods that could go unnoticed if only the total energy of the system was considered. In this regard, the…
In this study, we utilize the many-body expansion (MBE) framework to decompose electronic structures into fragments by incrementing the virtual orbitals. Our work aims to accurately solve the ground and excited state energies of each…
Facilitated by a rigorous partitioning of a molecular system's orbital basis into two fundamental subspaces - a reference and an expansion space, both with orbitals of unspecified occupancy - we generalize our recently introduced many-body…
A general polarizable embedded (PE) quantum mechanics/molecular mechanics scheme for periodic systems is presented, describing mutual polarization of the two subsystems. The QM system, described with density functional theory (DFT), is…
Energy-based fragmentation methods approximate the potential energy of a molecular system as a sum of contribution terms built from the energies of particular subsystems. Some such methods reduce to truncations of the many-body expansion…
In this second part of our series on the recently proposed many-body expanded full configuration interaction (MBE-FCI) method, we introduce the concept of multideterminantal expansion references. Through theoretical arguments and numerical…
Over the course of the past few decades, the field of computational chemistry has managed to manifest itself as a key complement to more traditional lab-oriented chemistry. This is particularly true in the wake of the recent renaissance of…
The many-body polarization energy is the major source of non-additivity in strongly polar systems such as water. This non-additivity is often considerable and must be included, if only in an average manner, to correctly describe the…
We investigate the coupling of different quantum-embedding approaches with a third molecular-mechanics layer, which can be either polarizable or non-polarizable. In particular, such a coupling is discussed for the multilevel families of…
We present a many-body expansion (MBE) formulation and implementation for efficient computation of analytical energy gradients from OSV-MP2 theory based on our earlier work (Zhou et al. J. Chem. Theory Comput. 2020, 16, 196-210). The…
Accurate many-body treatments of condensed-phase systems are challenging because correlated solvers such as full configuration interaction (FCI) and the density matrix renormalization group (DMRG) scale exponentially with system size.…
An approximate many-body theory incorporating two-body correlations has been employed to calculate low-lying collective multipole frequencies in a Bose-Einstein condensate containing $A$ bosons, for different values of the interaction…
The polarizable embedding (PE) model is a fragment-based quantum-classical approach aimed at accurate inclusion of environment effects in quantum-mechanical response property calculations. The aim of this tutorial is to give insight into…
Recent work has shown that the many-body expansion of the interaction energy can effectively be used to develop analytical representations of global potential energy surfaces (PESs) for water. In this study, the role of short- and…
The relative energies of different phases or polymorphs of molecular solids can be small, less than a kiloJoule/mol. Reliable description of such energy differences requires high quality treatment of electron correlations, typically beyond…
Polynomially filtered exact diagonalization method (POLFED) for large sparse matrices is introduced. The algorithm finds an optimal basis of a subspace spanned by eigenvectors with eigenvalues close to a specified energy target by a…